Metal organic frameworks (MOFs) are highly tailorable materials with proven ability for selective adsorption of gases. They can also be promising catalytic materials through covalently binding catalytic sites into the MOFs through post-synthetic modification, for example. We use a combination of density functional theory and statistical mechanical modeling to design MOFs that have the potential to both selectively adsorb CO2 capture from flue gas-like mixtures and that also have catalytic functional groups with high catalytic activity for converting CO2 to methanol and related molecules. We have screened many different potential catalytic materials in an effort to identify design principles for lowing the barriers of the reaction. One class of promising catalytic moieties are Lewis pairs, having both Lewis acid and base sites. For these functional groups the challenge is to selectively dissociate hydrogen rather than binding CO2. We show that geometric and topological constraints of the nanoporous framework are important in this regard. We also explore single metal atom catalysts as an alternative approach to Lewis pair functional groups. We find that there are different advantages and drawbacks to these two classes of catalytic functional groups.

Designing functionalized metal organic frameworks for carbon dioxide capture and hydrogenation

255th National Meeting (2018)

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